Breaking the symmetry of single-atom catalysts enables an extremely low energy barrier and high stability for large-current-density water splitting

被引:143
|
作者
Mu, Xueqin [1 ,2 ]
Gu, Xiangyao [1 ,3 ]
Dai, Shipeng [1 ]
Chen, Jiabing [1 ]
Cui, Yujia [1 ]
Chen, Qu [1 ]
Yu, Min [1 ]
Chen, Changyun [1 ]
Liu, Suli [1 ]
Mu, Shichun [2 ]
机构
[1] Nanjing Xiaozhuang Univ, Key Lab Adv Funct Mat Nanjing, Nanjing 211171, Peoples R China
[2] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
[3] Guangxi Normal Univ, Guangxi Key Lab Low Carbon Energy Mat, Guilin 541004, Peoples R China
基金
中国国家自然科学基金;
关键词
OXYGEN EVOLUTION; ELECTROCATALYSTS;
D O I
10.1039/d2ee01337a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The instability and low large-current-density efficiency for a single atomic metal species system have aroused widespread concern. Herein, the Ru single-atom system constructed on an iron-cobalt layered double hydroxide (Ru(x)SACs@FeCo-LDH) exhibits extremely low oxygen evolution reaction (OER) overpotentials of 194 and 246 mV at current densities of 10 and 1000 mA cm(-2), respectively, and a high stability greater than 1000 h at 1000 mA cm(-2), all of which far surpass the values obtained for commercial RuO2. Moreover, its mass activity is similar to 2 and 6 times higher than those of Ru and FeCo-LDH, respectively. Extraordinarily, it only needs 1.52 V to achieve a 1000 mA cm(-2) current density for water splitting, and it is almost unchanged after 1000 h, as the highest performance reported so far. Experimental and theoretical calculation results show that, after an activation process, an in situ Ru-O-TM (Fe, Co, and Ni)-like nanocompound is formed on the atom-scale symmetry breaking interfaces of the FeCo-LDH surface, promoting O-O coupling at the Ru-O active sites for OER and beneficial for suppressing multiple heteroatomic interface instability for large-current-density water splitting. Our strategy opens up opportunities for boosting the single-atom stability in industrial-scale hydrogen production from water splitting.
引用
收藏
页码:4048 / 4057
页数:10
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